Segmented Structure Design of Carbon Ring In-Plane Embedded in g-C3 N4 Nanotubes for Ultra-High Hydrogen Production

ChemSusChem. 2022 Oct 21;15(20):e202201268. doi: 10.1002/cssc.202201268. Epub 2022 Sep 13.

Abstract

The photocatalytic water splitting capability of metal-free graphitic carbon nitride (g-C3 N4 ) photocatalyst is determined by its microstructure and photoexcited electrons transfer. Herein, a segmented structure was developed, consisting of alternant g-C3 N4 nanotubes and graphitic carbon rings (denoted as Cr -CN-NT). The Cr -CN-NT showed ordered structure and ultralong length/diameter ratio of 150 nm in diameter and a few microns in lengths, which promoted electron transport kinetics and elongated photocarrier diffusion length and lifetime. Meanwhile, the local in-plane π-conjugation was formed and extended in Cr -CN-NT, which could improve charge carrier density and prohibit electron-hole recombination. Accordingly, the average hydrogen evolution rate of Cr -CN-NT reached 9245 μmol h-1 g-1 , which was 61.6 times that of pristine CN, and the remarkable apparent quantum efficiency (AQE) of Cr -CN-NT reached up to 12.86 % at 420 nm. This work may provide a pathway for simultaneous morphology regulation and in-plane modification of high-performance photocatalysts.

Keywords: carbon materials; graphitic carbon nitride; photocatalysis; water splitting; π-conjugation.